This dissertation presents experiments on nitrogen-vacancy (NV) defect centers in diamond. The NV center is an optically active color center formed by one substitutional nitrogen atom and an adjacent vacancy in the diamond lattice. Its ground state spin triplet transitions are accessible in the microwave regime and their corresponding excited state transitions exhibit spin-dependent fluorescence that allows for optical spin state readout. We present methods for the deterministic placement and the fine tuning of the NV center population in bulk diamond via ion implantation. We demonstrate quantum control of the nuclear spin in diamond through manipulation of the NV center electronic spin. By utilizing the hyperfine coupling between the electronic and nuclear spins, fast phase gates on the intrinsic nitrogen nuclear spin can be achieved within half a microsecond, a speed that far exceeds that of the gates performed with conventional nuclear magnetic resonance pulses. The hyperfine coupling also results in an enhancement of the effective nuclear gyromagnetic ratio. We demonstrate the tunability of this enhancement by changing the magnetic field. Finally, we discuss preliminary experiments aimed towards coupling a single NV center to higher nuclear spin systems.